Control of frictional interactions among liquid-suspended particles has led to tunable, strikingly non-Newtonian rheology the formation of strong flow constraints as particles come into close proximity under shear. Typically, these frictional interactions have been in the form of physical contact, controllable particle shape and surface roughness. We investigate a different route, where molecular bridging between nearby particle surfaces generates a controllable constraint to relative particle movement.
View Article and Find Full Text PDFSuspensions of polymeric nano- and microparticles are fascinating stress-responsive material systems that, depending on their composition, can display a diverse range of flow properties under shear, such as drastic thinning, thickening, and even jamming (reversible solidification driven by shear). However, investigations to date have almost exclusively focused on nonresponsive particles, which do not allow tuning of the flow properties. Polymeric materials possess rich phase transitions that can be directly tuned by their chemical structures, which has enabled researchers to engineer versatile adaptive materials that can respond to targeted external stimuli.
View Article and Find Full Text PDFThe non-Newtonian behaviors of dense suspensions are central to their use in technological and industrial applications and arise from a network of particle-particle contacts that dynamically adapt to imposed shear. Reported herein are studies aimed at exploring how dynamic covalent chemistry between particles and the polymeric solvent can be used to tailor such stress-adaptive contact networks, leading to their unusual rheological behaviors. Specifically, a room temperature dynamic thia-Michael bond is employed to rationally tune the equilibrium constant ( ) of the polymeric solvent to the particle interface.
View Article and Find Full Text PDFWe report on a nonequilibrium phase of matter, the minimally disordered crystal phase, which we find exists between the maximally amorphous glasses and the ideal crystal. Even though these near crystals appear highly ordered, they display glassy and jamming features akin to those observed in amorphous solids. Structurally, they exhibit a power-law scaling in their probability distribution of weak forces and small interparticle gaps as well as a flat density of vibrational states.
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